white paper describing COALA

COALA
Characterizing Organics and Aerosol Loading over Australia
WhitePaperforatroposphericchemistryfieldcampaigninSoutheastAustralia
Draft7July2016
SteeringGroup:
KathrynEmmerson(CSIRO)
JennyFisher,ClareMurphy,StephenWilson(U.Wollongong)
AlexGuenther(UC-Irvine)
LouisaEmmons,EricApel,ChristineWiedinmyer(NCAR)
etal…
Recenttechnologicaldevelopmentsnowmakeitpossibletofullyclosethe
reactivecarbonbudgetforisoprene,monoterpenesandsesquiterpenes,
includingquantifyingemissions,transformationsanddeposition.Thiswillallow
ustoaddressspecificquestionsrelatedtoamajoruncertaintyassociatedwith
climateforcing:knowinghowemissionswereprocessedinapristine
environmentrepresentativeofpre-industrialconditions.Theisolatedurban
areasofAustraliawillalsoallowustoquantifytheimpactofisoprene,
monoterpeneandsesquiterpeneemissionsonurbanairqualityandthe
emergingscienceoflowerNOxregimesinthematureindustrializedworldof
theNorthernHemisphere.
TableofContents
1. Introduction/ScientificRationale
2. KeyScienceQuestionsforCOALA
a. Emissions
b. Chemicalevolution
c. Climate&stresses
3. ExperimentalDesign
a. Ground-based
b. Aircraft
c. Satellites
4. Integrationwithmodels
5. Internationalcollaboration
6. References
COALAWhitePaperDraft7July2016
1
IntroductionandScientificRationale
Aquantitativedeterminationofthechangesinatmosphericchemistryandclimatesincepreindustrialtimesisurgentlyrequiredinordertodevelopeffectiveclimatemitigationand
adaptationstrategiesbutthisiscomplicatedbytheneedtocharacterizenaturalemission
sources,suchasthosefromundisturbedterrestrialvegetation,wildfire,andoceans,andthe
identificationofuniquechemicalprocesseswithouttheinfluencefromanthropogenicsources.
Largeareasofthesouthernhemisphere(SH)arenearpristineandprovideanopportunityto
investigatetheclean,naturalatmosphererelativelyfreeofanthropogenicinfluence,andthus
todefinethebaselinesfromwhichhumaninfluencescanbeassessed.Thisopportunityhas
largelybeenlostinthenorthernhemisphere(NH),andtheSHcouldserveasaproxyfor
potentialfutureconditionsinNorthAmerica(understricterpollutioncontrols).
SoutheastAustraliapresentsauniqueopportunitytoevaluatetheseprocesses.Estimatesof
BiogenicVolatileOrganicCompound(BVOC)emissionsbasedonmechanisticmodels(Arnethet
al.,2011;Guentheretal.,2012;Zengetal.,2015)andsatelliteobservations(Pfisteretal.2008)
showSoutheastAustralianbiogenicisopreneemissionsareamongthehighestintheworld
(Figure1),duelargelytotheprevalenceofdenselyforestedeucalyptecosystems.The
maximumemissionfactorinSoutheastAustraliais24000𝜇g/m2/hrwhichismorethandouble
theglobalaverageforanyPlantFunctionalType(11000𝜇g/m2/hr)fromGuentheretal(2012).
Eucalyptsalsoemitlargeamountsofmonoterpenesandsesquiterpenes(e.g.,Heetal.2000),
leadingtoacomplexmixofozoneandorganicaerosolprecursors.
However,modelsofBVOCemissionsinSEAustraliavarywidelyacrossinventories,with
differencesofafactorof2-3forisopreneandafactorof5-10formonoterpenes(Zengetal.,
2015;Sindelarovaetal.,2014;Emmersonetal,2016).Fieldobservationsofambient
concentrationsinvestigatedbyEmmersonetal.(2016)suggestthatisopreneemissionsare
overestimatedandmonoterpeneemissionsareunderestimated.Furthermore,themodel
predictionsofnearlyuniformisopreneandmonoterpeneemissionsacrosstheregion,asshown
inFigure1,areduetothesimplisticapproachforassigningemissionstoplantfunctionaltypes
andweexpectmuchhigherdiversityinrealitywithsomelandscapesdominatedby
monoterpenesandpossiblyevensesquiterpenes.Additionally,thechemistryoftheseemissions
ischallengingtosimulate.Forexample,formaldehyde(ahigh-yieldproductofisoprene
oxidation)inSEAustraliaisunderestimatedatWollongongby~50%irrespectiveofinventory
choice(Zengetal.,2015).
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Figure 1. Top and lower left: Isoprene emission factors from MEGAN (Guenther et al.,
2012). Lower right: emission factors for the sum of monoterpene species (α- and βpinene, limonene, carene, ocimene and sabinene).
AnthropogenicNOXemissionsinSEAustraliaareextremelylowandspatiallyisolated(Figure2),
withlittleanthropogenicinfluencesoutsidethemajorurbancentersofSydney,Canberra,and
Melbourne(NationalPollutantInventory:www.npi.gov.au).ThepopulationofAustraliais
denselylocatedinurbanhubsaroundthecoast,with90%ofpeoplelivingonjust0.22%ofthe
landarea(Sustainabilityreport,2013).TheisolationofanthropogenicNOxsourcesinSE
Australiameansthatthisregionprovidesanidealnaturallaboratorytostudytheimpactof
variableNOXamountsonBVOCchemistry(fromupwindofurbanareas,throughagradientat
theurbaninterface,tothedownwindoutflow).
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Figure 2. Tropospheric NO2 column from OMI satellite for July 2013 for Australia (left)
compared to the US (right). Australian fire activity is low at this time of year (NW
excepted), and NO2 amounts highlight the urban influences around the SE coast (Sydney,
Melbourne). Downloaded from KNMI/TEMIS.
Recentfieldcampaignsinvestigatedinteractionsbetweenbiogenicandanthropogenic
emissionsintheSoutheastUS(SOAS/SENEX/NOMADSS,SEAC4RS),wherebackgroundNOx
levelsarehigherandmuchlessspatiallydistinct(Figure2)andbiogenicemissionsare
dominatedbyisoprene.ThelowerbackgroundconcentrationsinAustraliawillallowstudies
targetingtheshiftfrommoderatetolow-NOxconditions.Thiswillprovideapreviewofthe
expectedfuturetrendsandconditionsintheU.S.andEurope,whereNOxlevelshavedeclined
sharplyinrecentyearsandareexpectedtocontinuedecreasinginresponsetostrengthenedair
qualityregulations(Duncanetal.,2016).Additionalrecentstudiesconductedintropicalforest
regionshaveexaminedbiogenic-anthropogenicemissionandchemicalinteractionsassociated
withanisolatedurbanplumeintheAmazonforest(GOAmazon)andoilpalmplantationsin
Borneo(OP3,Hewittetal.,2010)whicharebothregionswherebiogenicemissionsare
dominatedbyisoprene.Thesestudieshavedemonstratedtheimportanceofisoprene
emissionsindetermininganthropogenicimpactsbuthavealsoshownthatourcurrent
understandingisinsufficientforquantifyingtheimpactsandthattherearesubstantial
discrepanciesbetweenmodelsimulationsandobservations.TheCOALAresearchprogramwill
synthesizeknowledgefromtheserecentstudiesandapplyrecentadvancesinobservational
techniquesinordertoachieveacomprehensiveandsystematiccharacterizationofthereactive
carbonbudgetincludingemissions,depositionandatmospherictransformations.
TheCOALACampaign:
COALAwillbuildupontherecentadvancesinatmosphericchemistry,includingfieldcampaigns
thathavetakenplacearoundtheglobeinrecentyears,andwillfurthercharacterizeBVOC
emissions,chemistryandimplicationsforozoneandaerosolsinenvironmentwithvegetation
types,oxidantlevels,andclimateconditionsthatareunlikewhathaspreviouslybeen
investigated.InadditiontothemoderatetolowNOxconditionsinthisregion,thepresenceof
someeucalyptusforestswithrelativelyhighmonoterpeneemissionsandotherswithhigh
sesquiterpeneemissionsprovidesapotentialopportunitytocontrastregionsdominatedby
isoprenewithareasdominatedbymonoterpenesorevensesquiterpenes,unliketheprevious
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studiesincludingSOAS/SENEX/NOMADSS,SEAC4RS,OP3,GOAmazon).COALAisplannedfor
January-February2019,coordinatingflightsoftheU.S.NCAR/NSFC-130andU.K.FAAMBAe146
withground-basedandship-basedmeasurements.Apre-campaign(JOEY)isplannedfor
precedingsummers,andyear-roundmeasurementsatoneormorerepresentativegroundsites
willaimtocaptureseasonalvariations.
ThemeasurementsandmodelingassociatedwithCOALAwilladdresstheimpactsofchanging
biogenicemissionsduetoweatherextremesandclimatefactors.Sensitivitystudieswith
regionalandglobalcoupledchemistry-climatemodelswillexploretheimpactsofpossible
futureclimateconditions,suchasrisingtemperature,increasedfrequencyofdroughtand
temperatureextremes.Globalmodelsimulationswillalsoassistinquantifyingdifferences
betweenNorthernandSouthernHemispheresduetolowerCO2andCH4intheSH.Using
modelswithspecifieddynamicsallowsforsimulationofspecifictimeperiodsofpast
observationstotestandimprovebiogenicemissionsalgorithms,suchasMEGAN,under
stressedconditions.
TheCOALAcampaignwilladdressoneofthecentralthemesidentifiedattheAtmospheric
ChemistryCenterforObservationalResearchandData(ACCORD)CommunityWorkshop
(March2015,https://www2.acom.ucar.edu/accord/accord-2015-workshop),whichisto
conductafieldcampaigninaterpene-dominatedlandscapetoclosethereactivecarbon
budget.
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KeyScienceQuestionsforCOALA
Q1. How have emissions changed since pre-industrial conditions? Naturalemissions,fromundisturbedvegetation,wildlandfires,andmarinesources,controlled
thecompositionoftheatmosphereinpre-industrialtimes.Theseemissionshavecontinuedin
thepresenceofchangesinanthropogenicemissionsinthepast150years.Tounderstandthe
changesinchemistryandclimatesincepre-industrialtimes,itisrequiredtoquantifythe
emissionsoftracegasesandparticlesoverthistime.Todothis,severalspecificissuesneedto
beaddressed:
Q1A.WhatarethegaseousandparticulateemissionsfromnaturalsourcesinSEAustralia,
includingbiogenic,wildlandfire,andmarineemissions?
SoutheastAustraliahassignificantVOCandNOxemissionsfromterrestrialvegetation(both
undisturbedanddisturbed)aswellasfromwildlandfiresandfromthesurroundingoceans.Itis
essentialtoquantifytheemissionsfromthesesourcestopredictthechangesincomposition
sincepre-industrialtimesandclosethereactivecarbonbudgetoverthistime.Recentmodel
evaluationshaveshownsignificantdisagreementbetweenmodelsandobservationsdue,in
part,toerrorsinemissionsinventories.Forexample,Emmersonetal.(2016)showanoverestimateofisopreneemissions,butunder-estimateofterpeneemissions,insoutheast
Australia.FourdifferentglobalmodelsinarecentstudyalsodidapoorjobofreproducingCO
andformaldehydeobservationsintheSH,atleastinpartduetomisrepresentedemissions
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(Fisheretal.,2015;Zengetal.,2015).FluxtowermeasurementsinEucalyptforestover
extendedperiodswillallowquantificationofbiogenicVOCemissions.Additional
measurementsfromaircraftwillimproveestimatesofcanopy-scaleemissionsandwildfire(if
present)emissions.ThereissignificantuncertaintyoverDMSandVOCemissionsfromoceans
andship-basedandairbornemeasurementsovertheseawillassistinquantifyingthoseover
theSouthernOcean.
Q1B.Whatarethemagnitudeandtrendsofanthropogenicemissionsintheregion?
Thechemicalcompositionoftheatmospheresincepre-industrialtimeshaschangeddueinpart
totheincreasesandevolutionofanthropogenicemissions.Therefore,theseemissionsneedto
beelucidatedinordertoquantifyatmosphericcompositionoverthepast150years.Surface
measurementswithinthecitiesofsoutheastAustralia(Sydney,Melbourne,Brisbane),andover
powerplants,fossilfuelextractionandrefinerysitesandotherindustrialsites,ofsourcegases
andprimaryaerosols(CH4,CO,NOx,SO2,VOCs)willbeusedtoverifypresent-dayemissions
inventories.Long-termobservationsfromsurfacesitesandsatelliteswillbeusedtoestablish
pasttrends.
Bothground-basedandairbornemeasurementsofNOx,VOCsandaerosolconcentrationsand
fluxesoverSEAustraliacanquantifytheemissionsfrombiogenicandanthropogenicsources.
VOCemissionfluxeshavebeenquantifiedfrommeasurementsontheNCARC-130inpast
experiments(MIRAGE,NOMADSS,FRAPPÉ).Flighttracksofeitherracetracks,orstraightlegs
overuniformlandcover,atmultiplealtitudeswithintheboundarylayer,havebeenusedforflux
determination,andwouldcomplementtower-basedfluxmeasurementsinforestsforbiogenic
emissions(Karletal.,2009;Kaseretal.,2015).QuantificationofVOCemissionsovervarious
landscapesandtheoceanwouldbeachievedthroughlowaltitudeflights.
Q2. How are BVOC emissions chemically processed on local and regional
scales?
Anumberofquestionsremainregardingtheproductsandtheirrateofformationfrombiogenic
VOCsinlowNOxenvironments,particularlyfrommonoterpenesandsesquiterpenes.The
productionofozone,organicnitratesandsecondaryorganicaerosolshaveimportantimpacts
ondownwindairqualityaswellasradiationbudgets.
Q2A.Howdolow-NOxenvironmentsaffectthemechanismforBVOCoxidationinlocations
withsimilarconcentrationsofisopreneandterpenes,andhowdoesthisaffectsecondary
organicaerosolformation?
TheSEAustralianregionischaracterizedbylowbackgroundNOxconcentrations,withexisting
sourceslimitedtoafewspatiallydistincturbanareas(Fig.2),providingaclearNOxgradient
overwhichtoinvestigateanumberofrelatedquestionssurroundingisopreneandterpene
oxidation.OurcurrentunderstandingofBVOCchemicalprocessing(andsubsequentozoneand
aerosolformation)comesprimarilyfromareastargetedbypreviouscampaignswhereisoprene
dominatesobservedBVOCburdens(e.g.SoutheastUS,Amazon).InSEAustralia,isopreneand
monoterpenesarepresentatequalconcentrations(Emmersonetal.,2016).Theimpactsofthis
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muchlargerterpene-to-isopreneratioonatmosphericoxidizingcapacity,gas-phasechemical
processing,andorganicaerosolformationarenotknown.
TheOHradicalplaysacriticalroleinthischemistryastheinitiatorofVOCoxidationduringthe
day.However,thereisaseverelackofOHmeasurementsacrosstheSH.PreviousOH
measurementsinbiogenicenvironmentshavehighlightedmajorgapsinourunderstandingof
OHformationandrecyclingduringBVOCoxidation(e.g.,Lelieveldetal.,2008;Whalleyetal.,
2011).MeasurementsofOHandreactivityacrossdifferentNOxlevelsinSEAustraliawillhelp
furtherconstrainOHchemistryinthepresenceofsignificantterpeneconcentrations.
SOAformationinbalancedterpene-isopreneenvironmentshasnotbeenobservationally
constrained.SOAyieldsfrommonoterpenesarelargerthanfromisoprene.Inhigh-isoprene
environments,significantaerosolformationoccursvialow-NOxoxidationtoproduceisoprene
epoxydiols.However,thereissomeevidencethatisoprenedominancecansuppressaerosol
formation(Kanawadeetal.,2011).InSEAustralia,significantaerosolformationwasobserved
atnightatasitewithinadenseeucalyptforest(Tumbarumba)(Sunietal.,2008),butwithout
simultaneousgas-phaseobservations.Simultaneousobservationsofaerosolconcentration,
speciation,andgas-phaseprecursorsareneededtobetterunderstandaerosolformationin
terpene-isoprenebalancedenvironments.
Q2B.Howdoorganicnitratesforminhigh-BVOC,low-NOxenvironments,andwhatarethe
implicationsforNOx,ozone,andaerosols?
Organicnitratesexertasignificantinfluenceonthebudgetsofozone(Fioreetal,2005;
Horowitzetal.,2007)andorganicaerosols(Rollinsetal.,2013;Leeetal.,2016),bothwithin
sourceregionsandasameansforexportingNOx(viaPAN,forexample).Thereisevidencethat
formationoforganicnitratescanbetheprimarydeterminantoftheNOxlifetimeinlow-NOx
environments(BrowneandCohen,2012;Romeretal.,2016).However,inmosthigh-BVOC
regionsintheNH,anthropogenicNOxsourcesarespatiallydistributedacrossabackgroundof
highBVOCs,andverylittleofthelandscapehaslowenoughNOxemissionsfororganicnitrates
todominateNOxloss(Fisheretal.,2016).Whethersignificantorganicnitrateformationoccurs
inregionswhereNOxsourcesaresmallandisolatedremainsuncertain,asdotheimplications
forozoneandSOA.TheSEAustraliansettingwillallowustobetterconstrainpathwaysfor
organicnitrateformationandimpactsinlow-NOxenvironmentsandattheurban-rural
interface.ItwillalsoallowustotestwhetherNOxfromsoilsourcesorurbanoutflowcanlead
toorganicnitrateformationoverforests,andwhetherthisaffectsthelifetimeofNOxinthese
environments.
Q2C.TowhatextentdoesBVOCchemistrydriveairqualityincitiesdownwindofforests?
DenseanthropogenicNOxsourcesarespatiallyisolatedinAustraliaandsurroundedbysomeof
theworld’smostintensebiogenicsources.TheisolationofanthropogenicNOxsourcesinSE
Australiameansthatthisregionprovidesanidealnaturallaboratorytostudytheimpactof
variableNOXamountsonBVOCchemistry,fromupwindofurbanareas,throughagradientat
theurbaninterface,tothedownwindoutflow.OHdominatesoxidantchemistryduringthe
daytime,andusuallyquenchesmostisoprenebysunset.Isopreneremainingafterdarkis
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typicallyremovedbyreactionwithNO3radicals(Xieetal.,2013).However,whenNO3radical
formationissuppressed(asoccursinthepresenceofNOinurbanenvironments),isoprenecan
persistatnightanddrivemorningozoneformation(Milletetal.,2016).Throughthis
mechanismandthroughtheformationandtransportofBVOC-sourcedorganicaerosol,forests
cancontributetopoorairqualityincitiesdownwind.Citiesdownwindofforestsareprevalent
acrossthetropicsandtheSouthernHemisphere,andabetterunderstandingofthesebiogenicanthropogenicinteractionsattheforest-urbaninterfaceiscritical.
Q2D.CanisopreneemissionsbeinferredfromsatelliteHCHOinlowNOxconditions?
Isopreneemissionsarepoorlyconstrainedacrossmuchoftheglobe,particularlyinthetropics
andSH.Inmanyregionswhereinsituobservationsareunavailable,isopreneemissionsare
inferredusingsatelliteHCHOmeasurements(Kefauveretal.,2014,andreferencestherein).
However,lowNOxchemistrycanhindertheinterpretationofsatellitemeasurements.While
HCHOisproducedfrombothNOandHO2oxidation,theHCHOproductionratefromNO
oxidationismuchlarger.Asaresult,observedHCHOismorerepresentativeoflocalsurface
isoprenefluxesinregionswhereNOoxidationdominates.TheslowerHCHOproductioninlow
NOXregionscausespeakHCHOformationdownwindofisoprenesources.Thisleadsto
“smearing”oftheisoprene-HCHOrelationshipthatcanbealargesourceoferrorininferred
isopreneemissions(Palmeretal.,2003;Maraisetal.,2012;Barkleyetal.,2013).Whilethis
smearinghasbeenquantifiedtosomeextentundermoderatelylowNOXconditions,ithasnot
beenobservationallyconstrainedatverylowNOX(Wolfeetal.,2015).Suchconditionsare
representativeoflargeswathsoftheSH(Amazon,centralAfrica)thataretypicallydifficultto
reachandlogisticallychallengingformakingdedicatedmeasurements.Directcomparison
betweeninsituandsatellitemeasurementsarenecessarytounderstandthereliabilityofthe
satellitedataasaproxyforisopreneemissionsintheseregions(Zhuetal.,2016).
Q2E.WhatconditionscanweexpectinfuturefromdecliningNOxemissionsintheNH?
ThemuchlowerNOxbackgroundinSEAustraliarelativetotheNHmeansresultsfromthis
studymayprovideapreviewoftheexpectedfutureconditionselsewhere.IntheU.S.and
Europeinparticular,NOxlevelshavedeclinedsharplyinrecentyearsandareexpectedto
continuedecreasinginresponsetostrengthenedairqualityregulations(Duncanetal.,2016).
Theimplicationsforfutureorganicaerosolburdensremainuncertain,withmodelsshowing
conflictingresults.LowerNOxcanreduceorganicaerosolformationbyshuttingdownorganic
nitratemediatedchemistry(Pyeetal.,2015),butitcanalsoenhanceorganicaerosolformation
byshiftingmoreisopreneoxidationtothelow-NOxpathwayswithhigherSOAyields(Maraiset
al.,2016).ThelowNOxbackgroundsandstronggradientsofSEAustraliaprovidesanatural
laboratorytotestthesemodelsandidentifythedominanteffects,improvingourabilityto
predictfutureairqualityinNHcities.
Q3. How will climate change and extreme weather (e.g., drought and temperature
extremes) impact biogenic emissions? Solarradiation,temperatureandsoilmoistureconditionsareimportantforplantgrowth,and
non-optimalconditionssuchasdroughtmaytemporarilyincreaseBVOCemissionsbutwill
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ultimatelyinhibitemissions(Pegoraroetal2007;SharkeyandLoreto,1993).Australiahas
experiencedsignificantandlong-lastingdroughts,includingthe2001-2009MillenniumDrought
(Ummenhoferetal.,2009;vanDijketal.,2013),withimplicationsforbothvegetationcover
(especiallyleafareaindex;Huangetal.2014)andwaterstress,bothofwhichimpactBVOC
emissions(Fortunatietal.2008).Usingasoilmoistureactivityfactortoaccountfordrought
conditions,Sindelarovaetal.(2014)foundreductionsinisopreneemissionsofupto50%
globally,withevengreaterreductionsinregionsofAfricaandAustralia.
SoutheastAustraliaisalsoaregionwithhighsensitivitytoongoingglobalchange.Inthelast
decade,theregionhasexperiencedrecord-settingextremehightemperatures(LewisandKing,
2015),especiallyinsummer(LewisandKaroly,2013)whenBVOCemissionsreachtheirannual
peak.Isopreneemissionstypicallyincreasewithtemperature,butinatleastsomespeciesof
Eucalyptsisopreneemissionsflattenoutaround35°Candbegintodeclineattemperatures
above~40°C(Guentheretal.,1991;Pacificoetal.,2009).Dailymaximumtemperaturesinthis
rangecanoccurinsoutheastAustraliaduringsummer.DuringtheMeasurementofUrban,
MarineandBiogenicAircampaign(MUMBA)inthesummerof2012/2013,theairtemperature
surpassed40°Contwodays(Paton-Walshetal.,2016).HCHOobservationsfromWollongong
showlargeincreasesinaustralsummersince1997,especiallyduringseasonaltransitions(Nov,
Feb)thatmayindicatebiogenicemissionresponsetorisingtemperatureandlongergrowing
seasons(Lieschke,2015).
MeasurementsofmonoterpenesatTumbarumbainNovember2006showthecomplexeffects
ofplantstressonBVOCemissions.Anormalprofileshowstheexpectednighttimepeakin
monoterpeneconcentrationsduetolowmixingheightandchemicallossrates.However,under
stressconditionsafterasnowstormthemonoterpeneemissionsincreasedfour-fold,andthe
diurnalprofilelookedsimilartoisoprene,withamiddaypeak,whichsuggeststheemissionof
lightdependentmonoterpeneswhicharetypicallyassociatedwithstressinducedemissions
(Emmersonetal.,2016).
3
ExperimentalDesign
Anintensivefieldcampaignincludingaircraftandgroundstationsisplannedforaustralsummer
(January-February2019).BVOCemissionsareexpectedtopeakduringsummerwhenradiation
andtemperatureareattheirannualmaxima.Thesummertimingwillalsoprovidethe
possibilitytocaptureAustralianbiomassburningplumes(Edwardsetal.,2006).Inaddition,
ground-basedmeasurementshavebeenproposedforthesummersleadinguptothelarge
2019campaign.
3.1 Ground-&ship-basedmeasurements
Ground-andship-basedmeasurementswillcommencepriortothe2019intensivecampaign
andprovidealongertemporalspanofmeasurementsinseveraldifferentenvironments.Whilst
ground-basedmeasurementswillbeakeycomponentoftheintensive,theprinciplepurposeof
thiselementoftheprogrammeistoprovideadetailedcharacterisationofatmospheric
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compositionatafewsitespriortothemaincampaign.Thiswillprovideacontextualbasisfor
interpretingtheshorttemporalspanofmeasurementsoverthegreaterspatialextentcovered
bytheaircraftmeasurements.
Theground-basedmeasurementswillseektoquantifythemajorbiogenicVOCs,O3andNOXin
environmentsrelevantforthisproject:forestboundaries,urbanareas,andtheurban-forest
interface.Theship-bornemeasurementswillcharacterisebackgroundconcentrationsinclean
marineairandlatitudinalgradientsofbiogenicVOCs,O3andNOX.
Criticaltothesuccessofthisprojectiscollectionofhighqualityatmosphericobservationsatall
ofthefieldcampaigns.Tothisendgroundandship-bornemeasurementswillbeconducted
usingtheAtmosphericIntegratedResearchonBurdensandOxidativecapacity(AIR-BOX)facility
andancillaryinstrumentation.AIRBOXisacollaborativelyownedAustralianmobile
atmosphericlaboratory.Furtherdetailscanbefoundat:smah.uow.edu.au/cac/index.html.
WesternAir-ShedParticulateStudyforSydney(Jan-March2017)
ThefirstcampaignwillbeundertakenincollaborationwiththeCleanAirandUrbanLandscapes
hub(seewww.nespurban.edu.au),inWesternSydneyinearly2017.Thiscampaignisdesigned
toprovideobservationstotestanensembleofairqualitymodelsbeingdevelopedtoinform
policyoptionsforimprovedfutureairqualityoutcomesforSydney.
Specificaimsofthiscampaignareto:
• Quantifythecontributionofsecondaryorganicaerosolfrombiogenicand
anthropogenicsourcestoWesternSydneybyfusingreal-timeaerosolchemical
speciationdatawithstate-of-theartchemicaltransportmodelling
• Understandtheroleofnitrogenandsulphurchemistryintheformationofnewparticles
inWesternSydney.
Oakdale(summer2017-2018)
Thissecondcampaignisspecificallydesignedtocapturebiogenicemissionsclosetotheir
sourceinarurallocationtounderstandtheemissionsandformationofSOAawayfrommajor
anthropogenicinfluences(inalownitrogenoxidesenvironment).Thissiteissurroundedby
naturalbushland,betweentheNattaiNationalParktothewestandtheUpperNepeanState
ConservationAreatotheeast.TheproposedcampaignsiteisadjacenttoanexistingNewSouth
Walesairqualitymonitoringsite,whichcanprovidemeasurementsofairquality(includingfine
particleloadingbynephelometry)withhistoricalrecordsgoingbacktoJanuary1996.Themain
campaignwillbesupplementedbylongertermmeasurementsofVOCsatBargousingaPTR-MS
suppliedbytheUniversityofSydneyandisopreneusingachemiluminescenceinstrument
suppliedbyMacquarieUniversity.
Specificaimsofthiscampaignareto:
• QuantifythemajorbiogenicVOCsinforestboundaries
• IdentifywhichbiogenicVOCandoxidationproductsareofprimaryimportanceforSOA
generation.
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Brisbanesemi-ruralsite–Samfordvalley(summer2018-2019)
The3rdcampaignwillbelocatedsoastocapturebiogenicemissionsclosetourban
anthropogenicsources.QueenslandUniversityofTechnology(QUT)runandoperatedSamford
EcologicalResearchFacility(SERF)isanidealplaceforsuchmeasurements.SERFislocatedin
theSamfordValley,a25-minutedrivenorthwestofQUT’sGardensPointCampusinBrisbane,
Queensland.SimilartotheSydneystudytheaimsofthiscampaignareto:
• QuantifythemajorbiogenicVOCsinanurban/forestinterface
• Quantifythecontributionofsecondaryorganicaerosolfrombiogenicand
anthropogenicsourcestothesuburbanregionofBrisbanebyfusingreal-timeaerosol
chemicalspeciationdatawithstate-of-theartchemicaltransportmodelling
• Understandtheroleofnitrogenandsulphurchemistryintheformationandgrowthof
newparticlesinasubtropicalsuburbanarea
R.V.InvestigatorCampaigntoSampleCleanMarineAiratSouthernHemisphereMidlatitudes
Australia’snewmarinenationalfacility,theRVInvestigator,wouldhavethecapabilityto
characterisethecleanmarineairbackgroundconcentrationsandlatitudinalgradientsof
biogenicVOCs,O3andNOXatSHmid-latitudes.TheR.V.Investigatorhasabespokestainless
steelairsamplingtubethroughwhichairsamplescanbedrawnfrom6muptheforemastinto
thetwodedicatedlaboratoriesforatmosphericmeasurements.
Anaerosollaboratoryissituatedatthebow
directlybelowtheforemastandcontainsan
absorptionphotometer,anatmospheric
nephelometer,andascanningmobilityparticle
sizeraswellasaradondetector.Sampleairalso
passesthroughtheaerosollaboratoryandonto
thelargerairchemistrylaboratory,whichhouses
O3andNOXmonitorsaswellascavityring-down
spectrometersforCO2,CH4,COandN2O.Thereis
capacityforguestinstrumentsaboardtheR.V.
Investigator,eitherwithintheairchemistry
laboratoryorinsideashippingcontainer,whichmaybelocatedononeoftwopurpose
designedfootingsontheforedeck.Thetimingofthiscampaignissubjecttoavailabilityofshiptime.
Ongoingairqualitymonitoring
Inadditiontothemeasurementsdescribedabove,thereare42airqualitymonitoringstations
withinNewSouthWales,makingmeasurementsofPM10,PM2.5,O3,NOX,COandSO2,along
withmeteorologicalparameters(windspeed,winddirection,temperature,pressureand
relativehumidity).
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3.2 Aircraft
AircraftmeasurementswillbeakeycomponentofCOALA,providingregionalcontextand
linkingthevariousground-basedmeasurements.TheNCAR/NSFC-130hassuccessfullybeen
usedtoquantifyabove-canopybiogenicemissions(NOMADSS)andurban,agricultural,andoil
&gasexplorationemissions(FRAPPÉ).
DuringCOALA,theaircraftwillsamplealongtransectsspanningtheremoteforestedregions,
thepristinecoastalregionsandthecleanmarinebackground,aswellastheurbanizedcoastal
regionsaroundSydney,WollongongandMelbourne.Transectsthatsamplethedryinteriorand
drought-stressedregionswillalsobemadewherepossible.
TheNSF/NCARC-130andBAE146couldpotentiallybebasedattheIllawarraRegionalAirportin
AlbionPark,NewSouthWales(nearWollongong)(seeFigure4).Thiswouldbeagoodsite
becauseof:
- proximitytolikelygroundstations
- proximitytoSoutheasteucalyptforests
- abilitytosamplerangeofenvironmentsincludingdesert-agricultural-forestedsuburban-urban-oceanbyflyingeast-westtransects
- proximitytoUniversityofWollongongforinfrastructure/support
- lackofcommercialflightsshouldsimplifyflighttimingandairspaceconsiderations
Figure 3. Map of SE Australia.
3.3 Satellites
Satelliteobservationsoftroposphericconstituentsprovidelong-termandregional-to-global
contextfortheCOALAcampaign.ThelongtimerecordsfrominstrumentssuchasMOPITTand
OMIprovideaglobalclimatologyofCO,NO2,CH2O,O3,AOD,etc.,allowingquantificationofthe
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COALAWhitePaperDraft7July2016
seasonalcycleandvariability.Inturn,COALAground-basedandaircraftobservationswill
contributetothevalidationofthesatelliteretrievals.
SatelliteretrievalsofCO,fromMOPITTontheTerrasatellite(seeFigure5)andIASIonMetOpA
andMetOpB,willbeparticularlyvaluableduringCOALAtotracktheinfluenceofwildfire
emissionsoverAustralia.AerosolOpticalDepths(AOD)fromMODISonTerraandAquawill
alsoshowthelocationoffireplumesandpollutionoutflow.Satelliteretrievalsoftropospheric
NO2fromOMI(Figure2)andGOME-2highlightsourceregionssuchasurbancentersandwillbe
usefulfordeterminingwheretoflytobestintercepttherural-urbangradient.
SatelliteretrievalsarenowpossibleforseveralBVOCsandoxidationproducts,including
methanol,glyoxal,formicacid(IASI),andformaldehyde(OMIandGOME-2).Thesewillfacilitate
identificationofBVOCemissionsandtheirtemporalvariability(seeFigure6).Formaldehydein
particularhasbeenusedpreviouslytoquantifytheemissionofBVOCprecursorssuchas
isoprene.However,retrievingCH2Oamountsfromsatellitesisquitechallengingandrequires
extensiveaveragingtoestablishaclearsignal.ThereareknownbiasesincurrentCH2O
retrievals(Zhuetal.,2016),andtheisoprene-CH2Orelationshiphasnotbeenquantifiedina
high-terpeneenvironment.Thecoincidentground-based,airborne,andsatellitemeasurements
ofBVOCsandCH2Owillhelptobetterquantifysatellitebiasesandimproveunderstandingof
thelinksbetweenCH2OandBVOCfluxes.
Figure 4. Left: MOPITT CO surface retrieval for Jan 2016, with location of FTS sites.
Right: Wollongong FTS column CO time series with MOPITT CO, and weekly anomalies.
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COALAWhitePaperDraft7July2016
Figure 6. Monthly mean tropospheric HCHO columns from the OMI satellite, averaged
over Southeast Australia, with individual years in blue and multi-year means in black
(from Jesse Greenslade, University of Wollongong).
4
Integrationwithmodels
Chemistrymodelsacrossscalesfromboxmodelstoregionalandglobal3Dchemistry-climate
modelswillbeusedtodesignandinterprettheCOALAexperimentandresults.
Chemicalforecastsfromglobalandregionalmodels(suchasbeingprovidedforKORUS-AQ:
http://www.acom.ucar.edu/acresp/korus-aq/)willbeusedduringthecampaigntodetermine
flightplans.Near-real-timesimulationswillalsobecomparedtoearlyobservationsduringthe
campaign(asdonepreviouslyforSEAC4RS)tofurtherguideflightplanningbyidentifyingany
majorgapsbetweenmodelsandobservationsthatmaywarrantinvestigationinfutureflights.
Afterthecampaign,theaircraftandground-basedmeasurementswillbeusedtoevaluatethe
biogenicemissionsmodels(e.g.,MEGAN),theanthropogenicandwildfireemissions
inventories,andtherepresentationofchemicalprocessinginthemodels.Improvementswill
bemadetothemodels,asneeded,tobetterrepresenttheobservations.Themodelswillalso
beusedtoprovidecontextfortheobservations,suchasidentifyingwhenwildfireemissions
mayhaveimpactedtheobservations.
Coupledchemistry-climatemodelswillbetestedagainsttheCOALAobservationstoevaluate
themodels’abilitytoreproduceanatmospherestronglyinfluencedbybiogenicemissions,but
weaklybyanthropogenicsources.
5
Internationalcollaboration
COALAwillbringallthebenefitsofamajorinternationalcollaborativecampaign,with
involvementofresearchgroupsfromatleast3continents(America,EuropeandAustralia).
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COALAWhitePaperDraft7July2016
TheSteeringCommitteehasrepresentativesfromNCAR,UC-Irvine,CSIROandtheUniversityof
Wollongong,ensuringthatwithintheplanningstageCOALAhasbothresearchersexperienced
inrunningaircraftcampaignsandlocalrepresentatives,whocanorganizelogisticsonthe
ground.ThereisalsosignificantinterestinCOALAwithinEurope,withtheopportunityofthe
FAAMaircraftjoiningthecampaign.
TheuseofAIRBOXinthegroundcampaignwillinvolvealargeconsortiumofAustralian
universitiesandresearchinstitutes,includingtheUniversityofMelbourne,Queensland
UniversityofTechnology,MacquarieUniversity,theUniversityofWollongong,theUniversityof
Tasmania,MonashUniversity,theAustralianAntarcticDivision,theCommonwealthScientific
andIndustrialResearchOrganisationandAustralianNuclearScienceandTechnology
Organisation.OpportunitiesforresearcherstobehostedonboardoftheNCARC-130alsoexist.
Asignificantpartofthecollaborationwilloccuroncethecampaigndatahasbeencollected,
withthemanygroupssharingdata,coordinatingmodellingstudiesandworkingtogetherto
bestunderstand,analyseandpublishthefindingsfromthecampaign.Thiswillensurethatthe
resultsaredisseminatedtoawideanaudienceaspossible.
6
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